The Front Cover shows the utilization of benzimidazole-derivatized ligands and their mononuclear iron(III) complexes as a viable alternative for hydrolyzing organophosphate pesticides and also to evaluate the second coordination sphere effect of the benzimidazole moieties. Organophosphates are widely employed in safeguarding crops against pests and insects. However, due to their inherent toxicity, catalysts become imperative to facilitate their efficient degradation. The manuscript explores the investigation of the catalytic role played by benzimidazole groups, employing a comprehensive approach that encompasses experimental facets, as well as computational methods like DFT calculations. The findings skillfully strike a balance between the incorporation of aromatic-nucleophilic groups within the second coordination sphere and the optimization of side chain length in order to augment phosphoesterase activity. More information can be found in the Research Article by F. R. Xavier, R. A. Peralta, and co-workers.